银负载对活性炭纤维汞吸附性能的影响

银氨溶液浸渍活性炭纤维制得载银量14.07%的载银活性炭纤维.以筒状吸附体吸附气态Hg0的方式研究活性炭纤维银载前后的汞吸附性能,结果表明,载银后活性炭纤维汞吸附性能明显提高.实验还发现:随吸附温度升高,活性炭纤维的汞吸附效率随先增加后降低,而载银活性炭纤维的汞吸附效率随吸附温度升高而一直降低;延长停留时间和添加H2O(g)对两者汞吸附均有利.采用片状吸附体对2种吸附剂的汞饱和吸附量进行了测定,实验得出:70℃下活性炭纤维汞饱和吸附量为29.4 mg/g,载银活性炭纤维汞饱和吸附量为192.3 mg/g,即活性炭纤维载银后汞饱和吸附量提高到原来的6.54倍.扫描电镜分析发现:活性炭纤维上物理吸附汞占绝大多数,化学吸附汞很少;负载银后汞只吸附在活性炭纤维的含银活性点上,银粒子与汞结合生成银汞齐后形状趋于规则,且主要分布于活性炭纤维微晶的晶棱交界处.     

滤料负载粉尘层对气态汞脱除性能的实验研究

通过不同性能纤维滤料负载燃煤飞灰粉尘层,来模拟袋式除尘器滤袋表面粉尘附着层,进而研究袋滤器用不同性能纤维滤料和粉尘附着层对燃煤烟气中Hg0的联合脱除性能。在固定床实验系统上分别进行了不同纤维滤料和燃煤飞灰粉尘层,以及经实验优选得到的华博特滤料负载燃煤飞灰粉尘层脱除燃煤烟气中Hg0的实验研究。结果表明,燃煤飞灰粉尘层和华博特滤料对Hg0分别有一定的脱除作用,脱除效率可达35%和42.5%,它们对Hg0的脱除是物理吸附和化学吸附共同作用的结果;同时,华博特滤料负载燃煤飞灰粉尘层对Hg0的联合脱除效率受到吸附反应温度、入口汞浓度和烟气停留时间等因素的影响,最佳脱汞率可达64.4%;吸附反应温度越高,脱除效率越低;烟气停留时间越大,脱除效率越高;入口汞浓度的提高并不一定提高华博特滤料负载飞灰粉尘层的脱汞效果。     

ZnCl_2法污泥含炭吸附剂对模拟烟气中气态汞的吸附

采用改进的ZnCl2化学活化法制备污泥含炭吸附剂,利用EDS以及氮吸附等多种测试手段对所制得的污泥含炭吸附剂进行表征,并利用其处理模拟烟气汞污染物,实验结果表明,污泥含炭吸附剂对Hg0的吸附包括物理吸附作用和化学吸附作用,以物理吸附作用为主;随着Hg0入口浓度的提高,污泥含炭吸附剂的Hg0饱和吸附容量增大;随着吸附反应温度的升高污泥含炭吸附对Hg0的吸附作用减弱;在吸附反应温度125℃,Hg0入口浓度60.4 ug/m3,污泥含炭吸附剂和选定的活性炭对Hg0的吸附容量分别为81.2 ug/g和53.8 ug/g,污泥含炭吸附剂对Hg0的吸附作用好于选定的活性炭.     

ZnCl2法污泥含炭吸附剂对模拟烟气中气态汞的吸附

采用改进的ZnCl₂化学活化法制备污泥含炭吸附剂，利用EDS以及氮吸附等多种测试手段对所制得的污泥含炭吸附剂进行表征，并利用其处理模拟烟气汞污染物，实验结果表明，污泥含炭吸附剂对Hg0的吸附包括物理吸附作用和化学吸附作用，以物理吸附作用为主；随着Hg0入口浓度的提高，污泥含炭吸附剂的Hg0饱和吸附容量增大；随着吸附反应温度的升高污泥含炭吸附对Hg0的吸附作用减弱；在吸附反应温度125℃，Hg0入口浓度60.4 μg/m³，污泥含炭吸附剂和选定的活性炭对Hg0的吸附容量分别为81.2 μg/g和53.8 μg/g，污泥含炭吸附剂对Hg0的吸附作用好于选定的活性炭。     

载硫活性炭微观结构和表面形态研究

为了增强活性炭脱除燃煤电厂烟气中汞的能力，利用汞和硫可以生成稳定的HgS的性质，研究了通过热沉淀增加了活性炭中的硫含量的改性方法，并以SEM、BET、TGA等方法，研究了改性对活性炭表面形貌、硫在活性炭中的分布、活性炭比表面积等性能的影响。结果表明，热沉淀改性方法可以增加活性炭中的硫含量；硫粘附在活性炭的炭链上量较多，孔壁较少；改性工艺降低了活性炭的比表面积，且改性活性炭的比表面积随着温度的升高而增大；载硫后，活性炭中元素硫和炭的结合被增强。     

改性竹活性炭去除汞离子

采用溴化钾、碘化钾和硫磺对竹活性炭掺杂改性,利用电感耦合等离子体发射光谱仪测定滤液中汞离子浓度,用除汞效率和吸附容量评价活性炭对溶液中汞离子的吸附性能,探讨其吸附机理。结果表明,掺杂改性明显提高了竹活性炭的除汞性能。原竹活性炭的除汞效率为78.6%,吸附容量为2.210 mg/g;经碘化钾、溴化钾和硫磺掺杂改性后的竹活性炭除汞效率分别为94.3%、93.8%和88.8%,吸附容量分别为2.830、2.813和2.663 mg/g;经溴化钾(碘化钾)和硫磺联合改性的竹活性炭对水溶液中汞离子的吸附性能性能又有提高,其中以先载硫后载溴化钾的方法除汞效果最好,除汞效率达96.6%,吸附容量为2.898 mg/g。     

改性活性炭吸附净化黄磷尾气中的H2S

研究了以Cu2 离子活性溶液制备改性活性炭吸附净化黄磷尾气中H2S的相关问题,考察了改性活性炭制备过程中的浸渍液浓度、干燥温度和焙烧温度的影响,以及温度和氧含量对吸附的影响;并对空白活性炭、改性活性炭吸附前后做SEM表征.研究结果表明,浸渍液浓度0.05 mol/L、干燥温度120℃、焙烧温度250℃为改性活性炭制备的最佳条件;吸附反应阶段较适宜的温度为95℃,氧含量为1%;结合扫描电镜初步表明,改性后的活性炭S容量增加,吸附效果明显.     

废弃荧光灯中汞的处理

在30%的丙酮-水溶液中破碎废弃荧光灯,利用超声聚能效应辅助脱附汞,在有效捕获汞蒸气的同时脱附灯管表面大部分吸附汞。考察了丙酮水溶液浓度(C)、固液比(S/L)、超声时间(t)等因素对废弃荧光灯中汞去除效果的影响。在最佳工艺条件C=30%、S/L=240 g/L、t=30 min下,平均每根荧光灯中汞的去除量达5.028 mg。采用硫化沉淀-混凝-活性炭吸附联合工艺对含汞丙酮-水溶液进行无害化处理,实验结果表明,汞初始浓度为13.79 mg/L的废水,调节pH为2,依次投加硫化钠14.5 mg/L、聚合氯化铝290.9 mg/L、活性炭量90.9 mg/L,出水汞浓度降至26.82μg/L,去除率达99.8%,达到国家排放标准。     

改性活性炭吸附净化黄磷尾气中的H2S

研究了以Cu²⁺离子活性溶液制备改性活性炭吸附净化黄磷尾气中H₂S的相关问题，考察了改性活性炭制备过程中的浸渍液浓度、干燥温度和焙烧温度的影响，以及温度和氧含量对吸附的影响；并对空白活性炭、改性活性炭吸附前后做SEM表征。研究结果表明，浸渍液浓度0.05 mol/L、干燥温度120℃、焙烧温度250℃为改性活性炭制备的最佳条件；吸附反应阶段较适宜的温度为95℃，氧含量为1%；结合扫描电镜初步表明，改性后的活性炭S容量增加，吸附效果明显。     

CuCl_2改性材料脱除燃煤烟气中的Hg~0

烟气的脱汞治理已迫在眉睫。本研究以电厂燃煤锅炉废弃物飞灰和石灰为原料,丙酮溶液为分散剂制备了CuCl_2改性材料(CuCl_2-FS),并在固定床吸附评价装置上考察了CuCl_2改性对材料在模拟烟气中对Hg~0的脱除效果的影响。结果表明,经CuCl_2改性后对汞的脱除效率明显提高,并且温度的升高有利于提高其对烟气中Hg0的吸附性能。     

Enhanced mercuric chloride adsorption onto sulfur-modified activated carbons derived from waste tires

A number of activated carbons derived from waste tires were further impregnated by gaseous elemental sulfur at temperatures of 400 and 650 degrees C, with a carbon and sulfur mass ratio of 1:3. The capabilities of sulfur diffusing into the micropores of the activated carbons were significantly different between 400 and 650 degrees C, resulting in obvious dissimilarities in the sulfur content of the activated carbons. The sulfur-impregnated activated carbons were examined for the adsorptive capacity of gas-phase mercuric chloride (HgC1) by thermogravimetric analysis (TGA). The analytical precision of TGA was up to 10(-6) g at the inlet HgCl2 concentrations of 100, 300, and 500 microg/m3, for an adsorption time of 3 hr and an adsorption temperature of 150 degrees C, simulating the flue gas emitted from municipal solid waste (MSW) incinerators. Experimental results showed that sulfur modification can slightly reduce the specific surface area of activated carbons. High-surface-area activated carbons after sulfur modification had abundant mesopores and micropores, whereas low-surface-area activated carbons had abundant macropores and mesopores. Sulfur molecules were evenly distributed on the surface of the inner pores after sulfur modification, and the sulfur content of the activated carbons increased from 2-2.5% to 5-11%. After sulfur modification, the adsorptive capacity of HgCl2 for high-surface-area sulfurized activated carbons reached 1.557 mg/g (22 times higher than the virgin activated carbons). The injection of activated carbons was followed by fabric filtration, which is commonly used to remove HgCl2 from MSW incinerators. The residence time of activated carbons collected in the fabric filter is commonly about 1 hr, but the time required to achieve equilibrium is less than 10 min. Consequently, it is worthwhile to compare the adsorption rates of HgCl2 in the time intervals of < 10 and 10-60 min.     

Entrained-flow adsorption of mercury using activated carbon

Bench-scale experiments were conducted in a flow reactor to simulate entrained-flow capture of elemental mercury (Hg0) by activated carbon. Adsorption of Hg0 by several commercial activated carbons was examined at different C:Hg ratios (by weight) (350:1-29,000:1), particle sizes (4-44 microns), Hg0 concentrations (44, 86, and 124 ppb), and temperatures (23-250 degrees C). Increasing the C:Hg ratio from 2100:1 to 11,000:1 resulted in an increase in removal from 11 to 30% for particle sizes of 4-8 microns and a residence time of 6.5 sec. Mercury capture increased with a decrease in particle size. At 100 degrees C and an Hg0 concentration of 86 ppb, a 20% Hg0 reduction was obtained with 4- to 8-micron particles, compared with only a 7% reduction for 24- to 44-micron particles. Mercury uptake decreased with an increase in temperature over a range of 21-150 degrees C. Only a small amount of the Hg0 uptake capacity is being utilized (less than 1%) at such short residence times. Increasing the residence time over a range of 3.8-13 sec did not increase adsorption for a lignite-based carbon; however, increasing the time from 3.6 to 12 sec resulted in higher Hg0 removal for a bituminous-based carbon.     

Surface compositions of carbon sorbents exposed to simulated low-rank coal flue gases

Bench-scale testing of elemental mercury (Hg0) sorption on selected activated carbon sorbents was conducted to develop a better understanding of the interaction among the sorbent, flue gas constituents, and Hg0. The results of the fixed-bed testing under simulated lignite combustion flue gas composition for activated carbons showed some initial breakthrough followed by increased mercury (Hg) capture for up to approximately 4.8 hr. After breakthrough, the Hg in the effluent stream was primarily in an oxidized form (>90%). Aliquots of selected activated carbons were exposed to simulated flue gas containing Hg0 vapor for varying time intervals to explore surface chemistry changes as the initial breakthrough, Hg capture, and oxidation occurred. The samples were analyzed by X-ray photoelectron spectroscopy to determine changes in the abundance and forms of sulfur, chlorine, oxygen, and nitrogen moieties as a result of interactions of flue gas components on the activated carbon surface during the sorption process. The data are best explained by a competition between the bound hydrogen chloride (HCl) and increasing sulfur [S(VI)] for a basic carbon binding site. Because loss of HCl is also coincident with Hg breakthrough or loss of the divalent Hg ion (Hg2+), the competition of Hg2+ with S(VI) on the basic carbon site is also implied. Thus, the role of the acid gases in Hg capture and release can be explained.     

Adsorption of mercury by activated carbon prepared from dried sewage sludge in simulated flue gas

Conversion of sewage sludge to activated carbon is attractive as an alternative method to ocean dumping for the disposal of sewage sludge. Injection of activated carbon upstream of particulate matter control devices has been suggested as a method to remove elemental mercury from flue gas. Activated carbon was prepared using various activation temperatures and times and was tested for their mercury adsorption efficiency using lab-scale systems. To understand the effect of the physical property of the activated carbon, its mercury adsorption efficiency was investigated as a function of its Brunauer–Emmett–Teller (BET) surface area. Two simulated flue gas conditions, (1) without hydrogen chloride (HCl) and (2) with 20 ppm HCl, were used to investigate the effect of flue gas composition on the mercury adsorption capacity of activated carbon. Despite very low BET surface area of the prepared sewage sludge activated carbons, their mercury adsorption efficiencies were comparable under both simulated flue gas conditions to those of pinewood and coal activated carbons. After injecting HCl into the simulated flue gas, all sewage sludge activated carbons demonstrated high adsorption efficiencies, that is, more than 87%, regardless of their BET surface area.

Implications: We tested activated carbons prepared from dried sewage sludge to investigate the effect of their physical properties on their mercury adsorption efficiency. Using two simulated flue gas conditions, we conducted mercury speciation for the outlet gas. We found that the sewage sludge activated carbon had mercury adsorption efficiency comparable to pinewood and coal activated carbons, and the presence of HCl minimized the effect of physical property of the activated carbon on its mercury adsorption efficiency.     

Adsorption of elemental mercury vapors from synthetic exhaust combustion gas onto HGR carbon

An activated carbon commercially available named HGR, produced by Calgon-Carbon Group, was used to adsorbe metallic mercury. The work is part of a wider research activity by the same group focused on the removal of metallic and divalent mercury from combustion flue gas. With respect to previously published papers, this one is aimed at studying in depth thermodynamic equilibria of metallic mercury adsorption onto a commercial activated carbon. The innovativeness lies in the wider operative conditions explored (temperature and mercury concentrations) and in the evaluation of kinetic and thermodynamic data for a commercially available adsorbing material. In detail, experimental runs were carried out on a laboratory-scale plant, in which Hg° vapors were supplied in a nitrogen gas stream at different temperature and mercury concentration. The gas phase was flowed through a fixed bed of adsorbent material. Adsorbate loading curves for different Hg° concentrations together with adsorption isotherms were achieved as a function of temperature (120, 150, 200°C) and Hg° concentrations (1.0?7.0 mg/m³). Experimental runs demonstrated satisfying results of the adsorption process, while Langmuir parameters were evaluated with gas–solid equilibrium data. Especially, they confirmed that adsorption capacity is a favored process in case of lower temperature and they showed that the adsorption heat was –20 kJ/mol. Furthermore, a numerical integration of differential equations that model the adsorption process was proposed. Scanning electron microscopy (SEM) investigation was an useful tool to investigate about fresh and saturated carbon areas. The comparison between them allowed identification of surface sites where mercury is adsorbed; these spots correspond to carbon areas where sulfur concentration is greater.

Implications: Mercury compounds can cause severe harm to human health and to the ecosystem. There are a lot of sources that emit mercury species to the atmosphere; the main ones are exhaust gases from coal combustion and municipal solid waste incineration. Furthermore, certain CO₂ capture processes, particularly oxyfuel combustion in a pulverized fuel coal-fired power station, produce a raw CO₂ product containing several contaminants, mainly water vapor, oxygen, and nitrogen but also mercury, that have to be almost completely removed; otherwise these would represent a strong drawback to the success of the process.     

CuO-CeO2/AC吸附燃煤烟气中元素汞的实验研究

通过活性炭负载CuO和CeO2来制备吸附剂,采用固定床吸附方式,在不同反应条件下对吸附剂的吸附性能进行测试,筛选出去除效率最好的吸附剂,并通过BET和XRD对吸附剂的理化性质进行分析。结果表明,CuO和CeO2的加入大大改变了原活性炭的比表面积和孔结构,改善了活性炭的吸附性能。CuO-CeO2/AC中CuO和CeO2质量比不同,对汞的去除效率也不同,在1∶2时去除效率最好;CuO-CeO2/AC中所负载的CuO和CeO的总量为5%时,能大大促进汞的吸附效率,增长有效吸附时间;CuO-CeO2/AC对汞的吸附性能随反应温度的增加呈先增加后减小的趋势,在80℃时达到最大值。     

CuO-CeO_2/AC吸附燃煤烟气中元素汞的实验研究

通过活性炭负载CuO和CeO2来制备吸附剂,采用固定床吸附方式,在不同反应条件下对吸附剂的吸附性能进行测试,筛选出去除效率最好的吸附剂,并通过BET和XRD对吸附剂的理化性质进行分析。结果表明,CuO和CeO2的加入大大改变了原活性炭的比表面积和孔结构,改善了活性炭的吸附性能。CuO-CeO2/AC中CuO和CeO2质量比不同,对汞的去除效率也不同,在1∶2时去除效率最好;CuO-CeO2/AC中所负载的CuO和CeO的总量为5%时,能大大促进汞的吸附效率,增长有效吸附时间;CuO-CeO2/AC对汞的吸附性能随反应温度的增加呈先增加后减小的趋势,在80℃时达到最大值。     

Surface Compositions of Carbon Sorbents Exposed to Simulated Low-Rank Coal Flue Gases

Abstract

Bench-scale testing of elemental mercury (Hg⁰) sorption on selected activated carbon sorbents was conducted to develop a better understanding of the interaction among the sorbent, flue gas constituents, and Hg⁰. The results of the fixed-bed testing under simulated lignite combustion flue gas composition for activated carbons showed some initial breakthrough followed by increased mercury (Hg) capture for up to ～4.8 hr. After breakthrough, the Hg in the effluent stream was primarily in an oxidized form (>90%). Aliquots of selected activated carbons were exposed to simulated flue gas containing Hg⁰ vapor for varying time intervals to explore surface chemistry changes as the initial breakthrough, Hg capture, and oxidation occurred. The samples were analyzed by X-ray photoelectron spectroscopy to determine changes in the abundance and forms of sulfur, chlorine, oxygen, and nitrogen moieties as a result of interactions of flue gas components on the activated carbon surface during the sorption process. The data are best explained by a competition between the bound hydrogen chloride (HCl) and increasing sulfur [S(VI)] for a basic carbon binding site. Because loss of HCl is also coincident with Hg breakthrough or loss of the divalent Hg ion (Hg²⁺), the competition of Hg²⁺ with S(VI) on the basic carbon site is also implied. Thus, the role of the acid gases in Hg capture and release can be explained.     

Removal of carbonyl sulfide using activated carbon adsorption

Wastewater treatment plant odors are caused by compounds such as hydrogen sulfide (H2S), methyl mercaptans, and carbonyl sulfide (COS). One of the most efficient odor control processes is activated carbon adsorption; however, very few studies have been conducted on COS adsorption. COS is not only an odor causing compound but is also listed in the Clean Air Act as a hazardous air pollutant. Objectives of this study were to determine the following: (1) the adsorption capacity of 3 different carbons for COS removal; (2) the impact of relative humidity (RH) on COS adsorption; (3) the extent of competitive adsorption of COS in the presence of H2S; and (4) whether ammonia injection would increase COS adsorption capacity. Vapor phase react (VPR; reactivated), BPL (bituminous coal-based), and Centaur (physically modified to enhance H2S adsorption) carbons manufactured by Calgon Carbon Corp. were tested in three laboratory-scale columns, 6 in. in depth and 1 in. in diameter. Inlet COS concentrations varied from 35 to 49 ppmv (86-120 mg/m3). RHs of 17%, 30%, 50%, and 90% were tested. For competitive adsorption studies, H2S was tested at 60 ppmv, with COS at 30 ppmv. COS, RH, H2S, and ammonia concentrations were measured using an International Sensor Technology Model IQ-350 solid state sensor, Cole-Parmer humidity stick, Interscan Corp. 1000 series portable analyzer, and Drager Accuro ammonia sensor, respectively. It was found that the adsorption capacity of Centaur carbon for COS was higher than the other two carbons, regardless of RH. As humidity increased, the percentage of decrease in adsorption capacity of Centaur carbon, however, was greater than the other two carbons. The carbon adsorption capacity for COS decreased in proportion to the percentage of H2S in the gas stream. More adsorption sites appear to be available to H2S, a smaller molecule. Ammonia, which has been found to increase H2S adsorption capacity, did not increase the capacity for COS.